Article
Chemistry, Multidisciplinary
Hongsen Li, Zhengqiang Hu, Qingtao Xia, Hao Zhang, Zhaohui Li, Huaizhi Wang, Xiangkun Li, Fengkai Zuo, Fengling Zhang, Xiaoxiong Wang, Wanneng Ye, Qinghao Li, Yunze Long, Qiang Li, Shishen Yan, Xiaosong Liu, Xiaogang Zhang, Guihua Yu, Guo-Xing Miao
Summary: Research has found that cobalt oxide has larger storage capacity in lithium-ion batteries. The anomalous capacity is associated with the formation of a spin capacitor and the growth of a polymeric film. Operando magnetometry technology provides direct evidence of the catalytic role of metallic cobalt in assisting the polymeric film formation.
ADVANCED MATERIALS
(2021)
Article
Chemistry, Physical
Rhyz Pereira, Krishna Kumar Sarode, Ayda Rafie, Aaron Fafarman, Vibha Kalra
Summary: Lithium-sulfur batteries have potential challenges, but the use of sulfurized polyacrylonitrile (SPAN) and the presence of lithium nitrate can help retain capacity and suppress polysulfide formation by forming a robust cathode-electrolyte interphase.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Review
Chemistry, Physical
Wenzao Li, Diana M. Lutz, Lei Wang, Kenneth J. Takeuchi, Amy C. Marschilok, Esther S. Takeuchi
Summary: To overcome the limitations of static and destructive characterizations of Li-ion battery materials and components, a comprehensive investigation over various length and time scales is essential. Emerging in situ and operando characterization methodologies focusing on multiple size domains are a powerful approach to resolve current challenges and navigate future directions. The necessity and opportunity for in situ and operando characterization of electrochemical energy storage materials and systems are discussed, along with suggestions for future directions to tackle currently intractable issues on Li-ion battery application, failure, and emerging design concepts.
Review
Chemistry, Physical
Lanxin Xue, Yaoyao Li, Anjun Hu, Mingjie Zhou, Wei Chen, Tianyu Lei, Yichao Yan, Jianwen Huang, Chengtao Yang, Xianfu Wang, Yin Hu, Jie Xiong
Summary: This article summarizes the recent applications of in situ/operando Raman techniques for monitoring the real-time variations in Li-S batteries, aiming to reveal the reaction mechanism and guide the design of strategies for improving battery performances.
Review
Materials Science, Multidisciplinary
Feipeng Yang, Xuefei Feng, Y. -Sheng Liu, Li Cheng Kao, P. -A. Glans, Wanli Yang, Jinghua Guo
Summary: Researchers are aiming to develop alternative battery systems with low cost and high material abundance beyond lithium-ion batteries, emphasizing the importance of understanding the chemical and electronic structure of materials. Soft X-ray spectroscopy, as an element-specific technique, can be applied to study electronic and structural changes in electrode and electrolyte species through operando experiments, serving as a powerful tool for the development of beyond lithium-ion batteries.
ENERGY & ENVIRONMENTAL MATERIALS
(2021)
Article
Chemistry, Physical
Daniel Cordoba, Hernan B. Rodriguez, Ernesto J. Calvo
Summary: It has been discovered that the Li-O2 battery, which has the highest energy density comparable to fossil fuels, experiences parasitic reactions leading to degradation of the electrolyte and cathode material. These reactions limit the number of cycles due to the superoxide disproportionation that forms highly reactive singlet oxygen. This study introduces a novel in-operando method using a bifurcated optical fiber to detect singlet oxygen inside the battery during discharge. The detection is based on the reactivity of singlet oxygen with a fluorescent probe, which allows for real-time monitoring of singlet oxygen concentration. Additionally, the addition of azide ions, a well-known quencher of singlet oxygen, improves the cycling performance of Li-O2 batteries.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Andreas Strasser, Alexander Adam, Jiahao Li
Summary: Reducing the charging time is important for increasing the acceptance of electric vehicles. This paper introduces a new method that allows the detection of the onset of lithium plating in automotive lithium-ion batteries using online electrochemical impedance spectroscopy. The detection is based on observing the real part of the impedance across the state of charge during the charging procedure.
JOURNAL OF POWER SOURCES
(2023)
Article
Multidisciplinary Sciences
Alice J. Merryweather, Christoph Schnedermann, Quentin Jacquet, Clare P. Grey, Akshay Rao
Summary: The key to advancing lithium-ion battery technology, especially fast charging, lies in understanding dynamic processes in functioning materials under realistic conditions in real time. A laboratory-based optical interferometric scattering microscope was introduced to study nanoscopic lithium-ion dynamics in battery materials, allowing for high-throughput material screening. This methodology was applied to study various processes in battery materials, providing insights into battery degradation mechanisms.
Article
Chemistry, Multidisciplinary
Yun Seok Choi, Gwi Ok Park, Kyoung Ho Kim, Yelim Kwon, Joonsuk Huh, Ji Man Kim
Summary: The movement of sulfur species in the cathode of a lithium-sulfur battery was observed directly through operando SAXS analysis. Micropores serve as the primary repository for sulfur before and after the electrochemical reaction, while mesopores act as the actual reaction site for sulfur species. By establishing the distinct properties of the pores, critical insights were gained for the design of advanced carbon cathode materials.
CHEMICAL COMMUNICATIONS
(2021)
Article
Electrochemistry
M. A. Cabanero, M. Hagen, E. Quiroga-Gonzalez
Summary: High spatial resolution in-operando Raman spectroscopy was used to study lithium deposition on graphite electrodes, showing that lithium is deposited and intercalated into graphite simultaneously. After 30 minutes, a second mechanism becomes dominant. The evolution of G and D bands of graphite and the lithium concentration in the electrolyte suggest that EC is slowly consumed after lithium plating begins.
ELECTROCHIMICA ACTA
(2021)
Review
Chemistry, Multidisciplinary
Huibo Wang, De Ning, Litong Wang, Heng Li, Qingyuan Li, Mingzheng Ge, Junyan Zou, Shi Chen, Huaiyu Shao, Yuekun Lai, Yanyan Zhang, Guichuan Xing, Wei Kong Pang, Yuxin Tang
Summary: This review highlights the recent advances in the real-time investigation of lithium-ion batteries using neutron techniques. Neutron scattering, with its unique advantages, provides valuable insights into the battery mechanisms. Various neutron-based techniques have been applied in different scales and battery components.
Article
Multidisciplinary Sciences
Runlin Wang, Haozhe Zhang, Qiyu Liu, Fu Liu, Xile Han, Xiaoqing Liu, Kaiwei Li, Gaozhi Xiao, Jacques Albert, Xihong Lu, Tuan Guo
Summary: Understanding ion transport kinetics and electrolyte-electrode interactions is crucial for determining the performance and state of health of batteries. However, capturing the details of surface-localized and rapid ion transport at the microscale remains challenging. This study demonstrates a promising approach using an optical fiber plasmonic sensor to monitor the electrochemical kinetics of working batteries without disturbance, providing crucial additional capabilities to battery monitoring methods.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Lei Xu, Ye Xiao, Yi Yang, Shi-Jie Yang, Xiao-Ru Chen, Rui Xu, Yu-Xing Yao, Wen-Long Cai, Chong Yan, Jia-Qi Huang, Qiang Zhang
Summary: The relationship between electrical double layer capacitance and electrochemical active surface area of graphite anodes during Li-ion intercalation and Li plating processes is revealed. A lithium plating determination method based on dynamic capacitance measurement is proposed, which allows real-time monitoring of the onset of lithium plating in a working battery.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Lei Zhang, Qianwei Huang, Xiaozhou Liao, Yuhai Dou, Porun Liu, Mohammad Al-Mamun, Yun Wang, Shanqing Zhang, Shenlong Zhao, Dan Wang, Guowen Meng, Huijun Zhao
Summary: Yolk-shelled silicon/carbon materials show great promise as anode candidates for lithium-ion batteries, despite issues such as limited conductive promotion and low tap density. This study successfully synthesized a range of high-performance YS-Si/C anode materials and utilized an electrochemical transmission electron microscope system to gain insights into structural changes during battery operation, providing valuable guidance for the design of high-performance electrode materials.
ENERGY & ENVIRONMENTAL SCIENCE
(2021)
Article
Chemistry, Multidisciplinary
W. J. Legerstee, M. Boekel, S. Boonstra, E. M. Kelder
Summary: An Atomic Force Microscope (AFM) was combined with a special designed glovebox system and coupled to a Galvanostat/Potentiostat to allow measurements on electrochemical properties for battery research. The study found two dry methods to add lithium to the probe tip for use as an active element in measurements. The developed active probe method can be extended to techniques combining AFM measurements with mapping of electrochemical processes with spatial resolution.
FRONTIERS IN CHEMISTRY
(2021)
Article
Energy & Fuels
Thomas Waldmann, Rares-George Scurtu, Daniel Brandle, Margret Wohlfahrt-Mehrens
Summary: In this study, the tab design of Li-ion cells with the industrially relevant 21700 format was experimentally investigated. The effects of tab design on cell performance were observed through systematic variation of the tab design. The results showed that cells with a multitab design exhibited reduced impedance, improved charging rate capability, increased cycle stability, and enhanced charge throughput. X-ray computed tomography revealed that the improved cycle life was attributed to the reduction of inhomogeneities in the jellyrolls. Comparative analysis with cells from other studies provided insights into the magnitude of the effects of tab design variation.
Article
Energy & Fuels
Alice Hoffmann, Emanuel A. Heider, Christian Dreer, Claudia Pfeifer, Margret Wohlfahrt-Mehrens
Summary: The influence of industrial-suited mixing and dispersing processes on the processability, structure, and properties of suspensions and electrodes for lithium-ion batteries is examined, showing that the process strategy and shear stress strongly affect the properties of the suspensions and the microstructure, mechanical quality, and electrochemical performance of the resulting electrodes.
Article
Chemistry, Physical
S. Radloff, G. Carbonari, R. -G Scurtu, M. Hoelzle, M. Wohlfahrt-Mehrens
Summary: Substantial progress has been made in the lab-scale aqueous processing of Ni-rich cathode electrodes, and now it needs to be proven in production-scale to deliver competitive performance cells. This study successfully scaled up a carboxymethyl cellulose and styrene-butadiene rubber based electrode-coating recipe from lab-scale to production-scale, demonstrating homogeneous mass loading and excellent processability. Challenges such as slurry pH control and mixing/coating time adjustment were overcome. The pilot-scale cathode electrodes with high areal capacities were tested in pouch and cylindrical cells, showing promising capacity retention after thousands of cycles.
JOURNAL OF POWER SOURCES
(2023)
Article
Chemistry, Physical
Christin Hogrefe, Thomas Waldmann, Markus Hoelzle, Margret Wohlfahrt-Mehrens
Summary: Li metal deposition and internal short circuits in full cells are observed using in situ optical microscopy. Different conditions and effects, such as lithiation gradients, dendrite growth, dissolution rate, self-discharge, and the importance of separator pores, are discussed.
JOURNAL OF POWER SOURCES
(2023)
Article
Electrochemistry
Nicola Michael Jobst, Marilena Mancini, Markus Hoelzle, Margret Wohlfahrt-Mehrens, Peter Axmann
Summary: Nickel manganese spinel LiNi0.5Mn1.5O4 is a promising cobalt-free active material for lithium-ion battery cathodes due to its high operating voltage. However, extending the operating voltage range causes capacity fading, which is explained by the formation and re-transformation of a specific phase.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Energy & Fuels
Jonathan Schubert, Lukas Grossmann, Stefan Seidlmayer, Karl-Heinz Pettinger, Ralph Gilles, Michael A. Danzer
Summary: This study aims to identify the dominant active species in Saltwater Batteries with dual-ion electrolyte by conducting cyclic voltammetry and full cell measurements. The results show that the cathode only (de)intercalates lithium ions, while the anode can react with both sodium and lithium ions. However, lithium is found to be the dominant active species in the dual-ion battery.
Article
Electrochemistry
Erfan Moyassari, Simon Kuecher, Nicola Michael Jobst, Chia-Chin Chang, Shang-Chieh Hou, Franz B. Spingler, Margret Wohlfahrt-Mehrens, Andreas Jossen
Summary: During the charging or discharging of a lithium-ion battery (LIB), the volume of the electrodes can change due to lithiation or delithiation, which has a significant impact on the battery's lifetime. Factors such as initial porosity, particle shape, and silicon content affect the thickness change of various electrode materials.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Andreas Pfrang, Algirdas Kersys, Akos Kriston, Rares-George Scurtu, Mario Marinaro, Margret Wohlfahrt-Mehrens
Summary: The use of Si-containing negative electrodes is a promising option to increase the energy density of Li-ion batteries, but the challenge lies in managing the expansion/contraction behavior of Si during lithiation/de-lithiation. This study investigates the structural changes in Si-blended anode/manganese nickel cobalt oxide (NMC) 622 cathode 18650 format cells from production through end of life. It reveals the deformation mechanisms and the impact of cell geometry on the use and performance of high Si-content anodes.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Marius Fluegel, Marius Bolsinger, Mario Marinaro, Volker Knoblauch, Markus Hoelzle, Margret Wohlfahrt-Mehrens, Thomas Waldmann
Summary: Mixing graphite with Si particles in Li-ion battery anodes increases the specific energy, and higher Si contents result in thinner anode coatings with constant areal capacity. This study systematically investigates the influence of Si content on the susceptibility of Li plating on Si/graphite anodes.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Fabio Maroni, Min Li, Saustin Dongmo, Cornelius Gauckler, Margret Wohlfahrt-Mehrens, Marco Giorgetti, Mario Marinaro
Summary: In this study, iron hexacyanoferrate nanoparticles were synthesized using a microwave-assisted co-precipitation method, showing a specific capacity of 120 mAh g(-1) and a capacity retention of 84.8% over 100 cycles at 20 mA g(-1) current, as well as a capacity of 80 mAh g(-1) at 10 C rate. Ex-situ X-ray absorption spectroscopy (XAS) revealed some irreversibility and changes in Fe-C and Fe-N bond lengths during the initial charge/discharge cycle, which were attributed to electrode activation processes and partly explained the observed capacity fading.
Article
Engineering, Environmental
Zhen Chen, Hai-Peng Liang, Ziyuan Lyu, Neelima Paul, Giovanni Ceccio, Ralph Gilles, Maider Zarrabeitia, Alessandro Innocenti, Medina Jasarevic, Guk-Tae Kim, Stefano Passerini, Dominic Bresser
Summary: By using an ultrathin polysiloxane-based single-ion conductor (PSiO) as a multifunctional protection interlayer, the interfacial stability between LATP and Li-0 can be enhanced, effectively addressing the chemical instability issue of LATP. This approach improves the performance of solid-state lithium batteries.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Electrochemistry
Christin Hogrefe, Markus Hoelzle, Margret Wohlfahrt-Mehrens, Thomas Waldmann
Summary: In this study, the charging time was reduced by changing different cell- and charging parameters while keeping the cell chemistry unchanged. Through systematic experiments and optimization, methods and techniques for reducing the charging time under different conditions were obtained.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Nicola M. Jobst, Neelima Paul, Premysl Beran, Marilena Mancini, Ralph Gilles, Margret Wohlfahrt-Mehrens, Peter Axmann
Summary: This study investigates the dynamic evolution of the structure of high voltage spinel material LixNi0.5Mn1.5O4 using potentiostatic entropymetry, operando XRD, and neutron diffraction. The research reveals the distribution of lithium ions in the structure and provides explanations for the changes in battery performance.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
